Photoelectron angular distributions as a probe of alignment evolution in a polyatomic molecule: Picosecond time- and angle-resolved photoelectron spectroscopy of S1 para-difluorobenzene
Photoelectron angular distributions as a probe of alignment evolution in a polyatomic molecule: Picosecond time- and angle-resolved photoelectron spectroscopy of S1 para-difluorobenzene
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光电子角分布作为多原子分子排列演化的探针：S1 对二氟苯的皮秒时间和角度分辨光电子能谱
DOI：
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发表时间：
1999
期刊：
影响因子：
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通讯作者：
P. Matousek
中科院分区：
文献类型：
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作者：
K. L. Reid;T. Field;M. Towrie;P. Matousek
我们证明，皮秒时间分辨的光电子角分布（PAD）提供了一个敏感的探针的激发多原子分子的不断发展的对齐。这种演化的排列可以由纯旋转递归或旋转-振动耦合引起。如果选择的分子的旋转重现时间是众所周知的，该方法提供了一种建立分子内振动能量再分布（IVR）机制的方法。在S1对-二氟苯的情况下，我们观察到作为泵-探测时间延迟的函数的显著对准变化，我们将其归因于旋转介导的IVR。
We demonstrate that picosecond time-resolved photoelectron angular distributions (PADs) provide a sensitive probe of an evolving alignment in an excited polyatomic molecule. Such an evolving alignment can be caused by pure rotational recurrences or by rotation–vibration coupling. If a molecule is chosen for which the rotational recurrence times are well-known the method provides a means of establishing the mechanism of intramolecular vibrational energy redistribution (IVR). In the case of S1 para-difluorobenzene we observe striking alignment changes as a function of pump–probe time delay which we attribute to rotationally mediated IVR.